CN107039640B - Combination electrode material and its application - Google Patents
Combination electrode material and its application Download PDFInfo
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- CN107039640B CN107039640B CN201710121106.0A CN201710121106A CN107039640B CN 107039640 B CN107039640 B CN 107039640B CN 201710121106 A CN201710121106 A CN 201710121106A CN 107039640 B CN107039640 B CN 107039640B
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- 239000007772 electrode material Substances 0.000 title claims abstract description 63
- 229910001416 lithium ion Inorganic materials 0.000 claims abstract description 55
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims abstract description 53
- 239000007787 solid Substances 0.000 claims abstract description 53
- 239000003792 electrolyte Substances 0.000 claims abstract description 51
- 239000002994 raw material Substances 0.000 claims abstract description 40
- 230000000694 effects Effects 0.000 claims abstract description 30
- 239000000945 filler Substances 0.000 claims abstract description 21
- 239000006258 conductive agent Substances 0.000 claims abstract description 19
- 229910052744 lithium Inorganic materials 0.000 claims description 42
- 239000002253 acid Substances 0.000 claims description 40
- 239000000463 material Substances 0.000 claims description 36
- 239000002002 slurry Substances 0.000 claims description 34
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 33
- RJEIKIOYHOOKDL-UHFFFAOYSA-N [Li].[La] Chemical compound [Li].[La] RJEIKIOYHOOKDL-UHFFFAOYSA-N 0.000 claims description 33
- 239000002131 composite material Substances 0.000 claims description 28
- 239000007784 solid electrolyte Substances 0.000 claims description 22
- 238000000034 method Methods 0.000 claims description 16
- 239000000919 ceramic Substances 0.000 claims description 12
- 229910052715 tantalum Inorganic materials 0.000 claims description 12
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims description 12
- RIUWBIIVUYSTCN-UHFFFAOYSA-N trilithium borate Chemical compound [Li+].[Li+].[Li+].[O-]B([O-])[O-] RIUWBIIVUYSTCN-UHFFFAOYSA-N 0.000 claims description 9
- 229910002113 barium titanate Inorganic materials 0.000 claims description 8
- 239000010941 cobalt Substances 0.000 claims description 7
- 229910017052 cobalt Inorganic materials 0.000 claims description 7
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims description 7
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 6
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 6
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 6
- KFDQGLPGKXUTMZ-UHFFFAOYSA-N [Mn].[Co].[Ni] Chemical compound [Mn].[Co].[Ni] KFDQGLPGKXUTMZ-UHFFFAOYSA-N 0.000 claims description 6
- MRNHPUHPBOKKQT-UHFFFAOYSA-N indium;tin;hydrate Chemical group O.[In].[Sn] MRNHPUHPBOKKQT-UHFFFAOYSA-N 0.000 claims description 5
- 229910002097 Lithium manganese(III,IV) oxide Inorganic materials 0.000 claims description 4
- KLZUFWVZNOTSEM-UHFFFAOYSA-K Aluminum fluoride Inorganic materials F[Al](F)F KLZUFWVZNOTSEM-UHFFFAOYSA-K 0.000 claims description 3
- 229910002899 Bi2Te3 Inorganic materials 0.000 claims description 3
- 229910002903 BiCuSeO Inorganic materials 0.000 claims description 3
- 229910002971 CaTiO3 Inorganic materials 0.000 claims description 3
- 229910011557 Li4B2O5 Inorganic materials 0.000 claims description 3
- 229910013178 LiBO2 Inorganic materials 0.000 claims description 3
- 229910052493 LiFePO4 Inorganic materials 0.000 claims description 3
- 229910010881 LiInO2 Inorganic materials 0.000 claims description 3
- 229910017676 MgTiO3 Inorganic materials 0.000 claims description 3
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 3
- 239000004411 aluminium Substances 0.000 claims description 3
- 229910052782 aluminium Inorganic materials 0.000 claims description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 3
- WUKWITHWXAAZEY-UHFFFAOYSA-L calcium difluoride Chemical compound [F-].[F-].[Ca+2] WUKWITHWXAAZEY-UHFFFAOYSA-L 0.000 claims description 3
- 229910001634 calcium fluoride Inorganic materials 0.000 claims description 3
- 229910052681 coesite Inorganic materials 0.000 claims description 3
- 150000001875 compounds Chemical class 0.000 claims description 3
- 229910052593 corundum Inorganic materials 0.000 claims description 3
- 229910052906 cristobalite Inorganic materials 0.000 claims description 3
- 229910052909 inorganic silicate Inorganic materials 0.000 claims description 3
- 229910001386 lithium phosphate Inorganic materials 0.000 claims description 3
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 claims description 3
- 229910001635 magnesium fluoride Inorganic materials 0.000 claims description 3
- 229910052710 silicon Inorganic materials 0.000 claims description 3
- 239000010703 silicon Substances 0.000 claims description 3
- 239000000377 silicon dioxide Substances 0.000 claims description 3
- 229910052682 stishovite Inorganic materials 0.000 claims description 3
- 229910052712 strontium Inorganic materials 0.000 claims description 3
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 claims description 3
- 239000011366 tin-based material Substances 0.000 claims description 3
- 229910052905 tridymite Inorganic materials 0.000 claims description 3
- TWQULNDIKKJZPH-UHFFFAOYSA-K trilithium;phosphate Chemical group [Li+].[Li+].[Li+].[O-]P([O-])([O-])=O TWQULNDIKKJZPH-UHFFFAOYSA-K 0.000 claims description 3
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 3
- 241001481828 Glyptocephalus cynoglossus Species 0.000 claims description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 2
- 229910001453 nickel ion Inorganic materials 0.000 claims description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims 1
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims 1
- 229910052799 carbon Inorganic materials 0.000 claims 1
- 239000000758 substrate Substances 0.000 claims 1
- 229910052726 zirconium Inorganic materials 0.000 claims 1
- 239000000126 substance Substances 0.000 abstract description 13
- PQXKHYXIUOZZFA-UHFFFAOYSA-M lithium fluoride Chemical group [Li+].[F-] PQXKHYXIUOZZFA-UHFFFAOYSA-M 0.000 description 10
- 238000012360 testing method Methods 0.000 description 8
- 239000011149 active material Substances 0.000 description 6
- 229910052746 lanthanum Inorganic materials 0.000 description 6
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 6
- 239000002904 solvent Substances 0.000 description 6
- 238000002360 preparation method Methods 0.000 description 5
- 235000013399 edible fruits Nutrition 0.000 description 4
- 150000002500 ions Chemical class 0.000 description 4
- OAYXUHPQHDHDDZ-UHFFFAOYSA-N 2-(2-butoxyethoxy)ethanol Chemical group CCCCOCCOCCO OAYXUHPQHDHDDZ-UHFFFAOYSA-N 0.000 description 3
- 239000001856 Ethyl cellulose Substances 0.000 description 3
- ZZSNKZQZMQGXPY-UHFFFAOYSA-N Ethyl cellulose Chemical compound CCOCC1OC(OC)C(OCC)C(OCC)C1OC1C(O)C(O)C(OC)C(CO)O1 ZZSNKZQZMQGXPY-UHFFFAOYSA-N 0.000 description 3
- 230000008901 benefit Effects 0.000 description 3
- 239000011230 binding agent Substances 0.000 description 3
- 210000004027 cell Anatomy 0.000 description 3
- 230000000052 comparative effect Effects 0.000 description 3
- 239000002482 conductive additive Substances 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 229920001249 ethyl cellulose Polymers 0.000 description 3
- 235000019325 ethyl cellulose Nutrition 0.000 description 3
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 230000005012 migration Effects 0.000 description 3
- 238000013508 migration Methods 0.000 description 3
- 239000000203 mixture Substances 0.000 description 3
- 239000007773 negative electrode material Substances 0.000 description 3
- 238000011056 performance test Methods 0.000 description 3
- 239000007774 positive electrode material Substances 0.000 description 3
- 229910001220 stainless steel Inorganic materials 0.000 description 3
- 239000010935 stainless steel Substances 0.000 description 3
- JRPBQTZRNDNNOP-UHFFFAOYSA-N barium titanate Chemical compound [Ba+2].[Ba+2].[O-][Ti]([O-])([O-])[O-] JRPBQTZRNDNNOP-UHFFFAOYSA-N 0.000 description 2
- 239000003575 carbonaceous material Substances 0.000 description 2
- 239000006182 cathode active material Substances 0.000 description 2
- 210000001787 dendrite Anatomy 0.000 description 2
- 230000006872 improvement Effects 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 239000002105 nanoparticle Substances 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- -1 Li3InB2O6 Inorganic materials 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000005253 cladding Methods 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 230000005518 electrochemistry Effects 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 239000004744 fabric Substances 0.000 description 1
- 238000011031 large-scale manufacturing process Methods 0.000 description 1
- 229910003002 lithium salt Inorganic materials 0.000 description 1
- 159000000002 lithium salts Chemical class 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 239000003960 organic solvent Substances 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- 239000007790 solid phase Substances 0.000 description 1
- 230000006641 stabilisation Effects 0.000 description 1
- 238000011105 stabilization Methods 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
- H01M4/366—Composites as layered products
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
- H01M10/0562—Solid materials
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
- H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/628—Inhibitors, e.g. gassing inhibitors, corrosion inhibitors
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0065—Solid electrolytes
- H01M2300/0068—Solid electrolytes inorganic
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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- Condensed Matter Physics & Semiconductors (AREA)
- General Physics & Mathematics (AREA)
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- Crystallography & Structural Chemistry (AREA)
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Abstract
The invention discloses combination electrode material and its applications.Wherein, which includes: electrode active material, and the electrode active material includes: electrode activity raw material, and the electrode activity raw material is positive activated feedstock or negative electrode active raw material；Oxidate nano grain, the oxidate nano grain are distributed on the surface of the electrode activity raw material；Clad, the clad are coated on the electrode active material, and the clad includes: electrolyte；Inorganic nano-filler, the inorganic nano-filler are dispersed in the electrolyte；Conductive agent, the conductive agent are dispersed in the electrolyte.Have the characteristics that interface resistance is small, security performance is high, chemical stability is good, output energy density is high by the all-solid lithium-ion battery that the combination electrode material is prepared.
Description
Technical field
The present invention relates to field of energy source materials, and in particular, to combination electrode material and its application, more particularly, to
Combination electrode material, all-solid lithium-ion battery and the method for preparing all-solid lithium-ion battery.
Background technique
All-solid lithium-ion battery is because it is with high security performance, high-energy density, excellent electrochemical stability etc.
Advantage and concern by more and more people.All-solid lithium-ion battery is mainly by solid anode, solid electrolyte, solid cathode
Three parts composition, compared with commercial lithium battery, solid electrolyte material plays lithium salts, organic solvent and diaphragm three parts simultaneously
Effect hinder the growth of Li dendrite to simplify the structure of battery so as to improve the safety of battery.In addition, Quan Gu
State lithium battery can be expected to be applied to the neck such as MEMS and micro drives power supply by fixing fabric structure in lesser scale
Domain.At present all-solid lithium-ion battery include film-type all-solid lithium-ion battery and figure all-solid lithium-ion battery,
The extensive industrialization process of middle film-type all-solid lithium-ion battery is hampered by that its energy density is small, active material bearing capacity
Low, the disadvantages of preparation cost is sufficiently expensive.And figure all-solid lithium-ion battery due to its huge interface resistance but also its
It can not carry out large-scale industrialized production.
All-solid lithium-ion battery requires study as a result,.
Summary of the invention
The present invention is directed at least solve one of the technical problems existing in the prior art.For this purpose, one object of the present invention
It is to propose a kind of combination electrode material that there is interface using the all-solid lithium-ion battery that the combination electrode material is prepared
The features such as resistance is small, security performance is high, chemical stability is good, output energy density is high.
According to an aspect of the present invention, the present invention devises a kind of new combination electrode material.Reality according to the present invention
Example is applied, which includes: electrode active material, and the electrode active material includes: electrode activity raw material, the electricity
Pole activated feedstock is positive activated feedstock or negative electrode active raw material；Oxidate nano grain, the oxidate nano grain are distributed in institute
On the surface for stating electrode activity raw material；Clad, the clad are coated on the electrode active material, the clad packet
It includes: electrolyte；Inorganic nano-filler, the inorganic nano-filler are dispersed in the electrolyte；Conductive agent, it is described
Conductive agent is dispersed in the electrolyte.
Combination electrode material according to an embodiment of the present invention, wherein electrode active material is provided as lithium source supplying party can
With the lithium ion of migration, the oxidate nano grain of electrode activity stock chart EDS maps can reduce lithium ion in electrode activity raw material
Resistance when migrating with the interface of electrolyte, reduces the interface resistance of battery；Electrolyte can promote compound electric
The conduction of extremely middle lithium ion, conductive agent can promote the conduction of electronics in combination electrode；Inorganic nano-filler can reduce lithium from
The resistance that son migrates inside electrolyte and between electrode activity raw material and the interface of electrolyte, reduces battery
Resistance.The all-solid lithium-ion battery interface resistance formed in turn using the combination electrode material is small, security performance is high, chemical steady
Qualitative good, output energy density height.
In addition, combination electrode material according to the above embodiment of the present invention can also have the following additional technical features:
According to an embodiment of the invention, the mass fraction of the clad is 1-10%.
According to an embodiment of the invention, the quality of the electrolyte, the inorganic nano-filler and the conductive agent
Than for (10-30): (2-20): (2-20).
According to an embodiment of the invention, the positive-active raw material is selected from cobalt acid lithium, LiMn2O4, nickel-cobalt-manganese ternary material
Material, at least one of nickel ion doped, nickel cobalt manganese richness lithium ternary material and LiFePO4.
According to an embodiment of the invention, the negative electrode active raw material be selected from carbon-based material, silica-base material, tin-based material,
At least one of lithium titanate or lithium metal.Preferred embodiment in accordance with the present invention, the negative electrode active raw material are lithium metal.
According to an embodiment of the invention, the oxidate nano grain is selected from Al2O3、ZrO2、SiO2、BaTiO3、CaTiO3、
MgTiO3And MgOAl2O3At least one of.Preferred embodiment in accordance with the present invention, the oxidate nano grain are
BaTiO3。
According to an embodiment of the invention, the electrolyte is selected from Li3PO4、Li4SiO4、Li3BO3、Li4B2O5、
LiInO2、Li3InB2O6、LiBO2At least one of.Preferred embodiment in accordance with the present invention, the electrolyte are
Li3BO3。
According to an embodiment of the invention, the inorganic nano-filler is selected from LiF, CaF2、MgF2、LiI、AlF3And LiBF4
At least one.Preferred embodiment in accordance with the present invention, the inorganic nano-filler are LiF.
According to an embodiment of the invention, the conductive agent is In2O5(Sn)、Bi2Te3、Cu2Se, BiCuSeO and Ni1-x
(Lix)O2At least one of.Preferred embodiment in accordance with the present invention, the conductive agent are In2O5(Sn)。
According to another aspect of the invention, the present invention provides a kind of all-solid lithium-ion batteries.Reality according to the present invention
Example is applied, which includes: plus plate current-collecting body；Anode layer, the anode layer include combination electrode material above-mentioned
Material, wherein electrode activity raw material is positive activated feedstock；Solid-state electrolyte layer；Negative electrode layer, the negative electrode layer include above-mentioned multiple
Composite electrode material, wherein electrode activity raw material is cathode activated feedstock；And negative current collector.
The all-solid lithium-ion battery of embodiment according to the present invention is formed complete solid using combination electrode material above-mentioned
State lithium ion battery has the characteristics that security performance is high, chemical stability is good, and this new combined electrode structure is improving electrode
While active material bearing capacity, increase battery energy density, the interface resistance of battery, while battery are effectively reduced
Preparation method is very simple, cheap, efficient, is suitble to large-scale industrialized production.
According to an embodiment of the invention, the anode layer with a thickness of 20-30 μm.
According to an embodiment of the invention, the negative electrode layer with a thickness of 20-30 μm.
According to an embodiment of the invention, the solid-state electrolyte layer is made of zirconic acid lanthanum lithium-based ceramic.
According to an embodiment of the invention, the zirconic acid lanthanum lithium-based ceramic is selected from zirconic acid lanthanum lithium, strontium doping zirconic acid lanthanum lithium, tungsten
It adulterates in zirconic acid lanthanum lithium, tantalum doping zirconic acid lanthanum lithium, Ge-doped zirconic acid lanthanum lithium, aluminium doping zirconic acid lanthanum lithium and silicon doping zirconic acid lanthanum lithium
It is at least one.Preferred embodiment in accordance with the present invention, the zirconic acid lanthanum lithium-based ceramic are that tantalum adulterates zirconic acid lanthanum lithium.
According to an embodiment of the invention, the all-solid lithium-ion battery is in laminated.
In accordance with a further aspect of the present invention, the present invention provides a kind of sides for preparing all-solid lithium-ion battery above-mentioned
Method.According to an embodiment of the invention, this method comprises: prepare composite positive pole slurry and composite negative pole material slurry, it is described
Composite positive pole slurry contains the raw material to form the predetermined amount of anode layer, and the composite negative pole material slurry contains to form cathode
The raw material of the predetermined amount of layer；Form solid-state electrolyte layer；Utilize the composite positive pole slurry and the composite negative pole material
Slurry forms anode layer and negative electrode layer in the both side surface of the solid-state electrolyte layer；In the anode layer and the negative electrode layer
Surface be respectively formed plus plate current-collecting body and negative current collector, to obtain the all-solid lithium-ion battery.Utilizing as a result, should
The all-solid lithium-ion battery of method preparation, security performance is high, and chemical stability is good, output power is high.
According to an embodiment of the invention, the composite positive pole slurry and the composite negative pole material slurry are printed respectively
Brush is in the both side surface of the solid-state electrolyte layer and is heat-treated, and anode layer and negative electrode layer are formed.
According to an embodiment of the invention, the solid-state electrolyte layer is ceramic solid electrolyte layer.
Additional aspect and advantage of the invention will be set forth in part in the description, and will partially become from the following description
Obviously, or practice through the invention is recognized.
Detailed description of the invention
Above-mentioned and/or additional aspect of the invention and advantage will become from the description of the embodiment in conjunction with the following figures
Obviously and it is readily appreciated that, in which:
Fig. 1 shows the charge and discharge knot of all-solid lithium-ion battery according to an embodiment of the invention at room temperature
Fruit schematic diagram；
Fig. 2 shows the charge and discharge knot of all-solid lithium-ion battery according to an embodiment of the invention at room temperature
Fruit schematic diagram；
Fig. 3 shows the charge and discharge knot of the all-solid lithium-ion battery of a comparative example according to the present invention at room temperature
Fruit schematic diagram.
Specific embodiment
The embodiment of the present invention is described below in detail, examples of the embodiments are shown in the accompanying drawings, wherein from beginning to end
Same or similar label indicates same or similar element or element with the same or similar functions.Below with reference to attached
The embodiment of figure description is exemplary, and for explaining only the invention, and is not considered as limiting the invention.
In the description of the present invention, term " longitudinal direction ", " transverse direction ", "upper", "lower", "front", "rear", "left", "right", " perpendicular
Directly ", the orientation or positional relationship of the instructions such as "horizontal", "top", "bottom" is to be based on the orientation or positional relationship shown in the drawings, and is only
For ease of description the present invention rather than require the present invention that must be constructed and operated in a specific orientation, therefore should not be understood as pair
Limitation of the invention.
It should be noted that term " first ", " second " are used for description purposes only, it is not understood to indicate or imply phase
To importance or implicitly indicate the quantity of indicated technical characteristic.Define " first " as a result, the feature of " second " can be with
Explicitly or implicitly include one or more of the features.Further, in the description of the present invention, unless otherwise saying
Bright, the meaning of " plurality " is two or more.
According to an aspect of the present invention, the present invention provides a kind of combination electrode materials.According to an embodiment of the invention,
The combination electrode material includes: electrode active material and clad.According to an embodiment of the invention, electrode active material includes:
Electrode activity raw material and oxidate nano grain, wherein electrode activity raw material is positive activated feedstock or negative electrode active raw material；Oxidation
Object nanoparticle is distributed on the surface of electrode activity raw material.According to an embodiment of the invention, clad is coated on electrode activity material
On material, which includes: electrolyte, inorganic nano-filler and conductive agent, inorganic nano-filler and conductive agent Monodispersed
In the electrolyte, further, inorganic nano-filler and conductive agent are in Dispersed precipitate.
Combination electrode material according to an embodiment of the present invention, wherein electrode active material is provided as lithium source supplying party can
With the lithium ion of migration, the oxidate nano grain of electrode activity stock chart EDS maps can reduce lithium ion in electrode activity raw material
Resistance when migrating with the interface of electrolyte, reduces the interface resistance of battery；Electrolyte can promote compound electric
The conduction of extremely middle lithium ion, conductive agent can promote the conduction of electronics in combination electrode；Inorganic nano-filler can reduce lithium from
The resistance that son migrates inside electrolyte and between electrode activity raw material and the interface of electrolyte, reduces battery
Resistance.And then it is high using the all-solid lithium-ion battery security performance that the combination electrode material is formed, chemical stability is good, exports
Power is high.
According to an embodiment of the invention, the mass fraction of clad is 1-10%.Lithium ion is in combination electrode as a result,
Stable migrating channels are formed, cell resistance is lower.
According to an embodiment of the invention, the mass ratio of electrolyte, inorganic nano-filler and conductive agent is (10-30):
(2-20): (2-20).Solid electrolyte/electrode active material interface compatibility is good as a result, combination electrode material intermediate ion
Conductibility is high, and electro-chemical activity is high.
According to an embodiment of the invention, positive-active raw material is selected from cobalt acid lithium, LiMn2O4, nickel-cobalt-manganese ternary material, nickel
At least one of LiMn2O4, nickel cobalt manganese richness lithium ternary material and LiFePO4.Solid state battery capacity is high as a result, and electrochemistry is living
Property is good.
According to an embodiment of the invention, negative electrode active raw material is selected from carbon-based material, silica-base material, tin-based material, metatitanic acid
At least one of lithium or lithium metal.Preferred embodiment in accordance with the present invention, the negative electrode active raw material are lithium metal.As a result,
Solid state battery capacity is high, and electro-chemical activity is good.
According to an embodiment of the invention, oxidate nano grain is selected from Al2O3、ZrO2、SiO2、BaTiO3、CaTiO3、
MgTiO3And MgOAl2O3At least one of.Preferred embodiment in accordance with the present invention, oxidate nano grain are BaTiO3.By
This, lithium ion is substantially reduced in solid electrolyte/electrode active material interfacial migration resistance, and cell resistance is substantially reduced.
According to an embodiment of the invention, electrolyte is selected from Li3PO4、Li4SiO4、Li3BO3、Li4B2O5、LiInO2、
Li3InB2O6、LiBO2At least one of.The conductibility of combination electrode material intermediate ion is good as a result,.It is according to the present invention preferred
Embodiment, electrolyte Li3BO3.The conductibility of combination electrode material intermediate ion is more preferably as a result,.
According to an embodiment of the invention, inorganic nano-filler is selected from LiF, CaF2、MgF2、LiI、AlF3And LiBF4Extremely
Few one kind.The improvement of solid electrolyte/electrode active material interface compatibility is good as a result,.It is according to the present invention preferred
Embodiment, the inorganic nano-filler are LiF.The improvement effect of solid electrolyte/electrode active material interface compatibility as a result,
More preferably, durability is good for fruit, and electro-chemical activity is high.
According to an embodiment of the invention, conductive agent is In2O5(Sn)、Bi2Te3、Cu2Se, BiCuSeO and Ni1-x(Lix)O2
At least one of.The conductibility of combination electrode material intermediate ion is good as a result,.Preferred embodiment in accordance with the present invention, it is described to lead
Electric agent is In2O5(Sn).The conductibility of electronics is good in combination electrode material as a result, and electro-chemical activity is high.
According to another aspect of the invention, the present invention provides a kind of all-solid lithium-ion batteries.Reality according to the present invention
Example is applied, which includes: plus plate current-collecting body, anode layer, solid-state electrolyte layer, negative electrode layer and negative pole currect collecting
Body.According to an embodiment of the invention, anode layer includes combination electrode material above-mentioned, wherein electrode activity raw material is that anode is living
Property raw material；Negative electrode layer includes combination electrode material above-mentioned, wherein electrode activity raw material is cathode activated feedstock.
The all-solid lithium-ion battery of embodiment according to the present invention is formed complete solid using combination electrode material above-mentioned
State lithium ion battery has the characteristics that security performance is high, chemical stability is good, and this new combined electrode structure is improving electrode
While active material bearing capacity, increase battery energy density, the interface resistance of battery, while battery are effectively reduced
Preparation method is very simple, cheap, efficient, is suitble to large-scale industrialized production.According to an embodiment of the invention, the battery can be with
It uses at a room temperature and a high temperature.
According to an embodiment of the invention, anode layer with a thickness of 20-30 μm.The thickness of anode layer is big as a result, active material
Bearing capacity is big, and output energy density is high.
According to an embodiment of the invention, negative electrode layer with a thickness of 20-30 μm.The thickness of negative electrode layer is big as a result, active material
Bearing capacity is big, and output energy density is high.
According to an embodiment of the invention, solid-state electrolyte layer is made of zirconic acid lanthanum lithium-based ceramic.Cell safety as a result,
Property is good, has prevented the security risks such as leakage, Li dendrite.
Wherein, it should be noted that in the present invention, the electrolyte in the raw material and electrode material of solid-state electrolyte layer
For different materials.
According to an embodiment of the invention, zirconic acid lanthanum lithium-based ceramic is selected from zirconic acid lanthanum lithium, strontium doping zirconic acid lanthanum lithium, witch culture
In zirconic acid lanthanum lithium, tantalum doping zirconic acid lanthanum lithium, Ge-doped zirconic acid lanthanum lithium, aluminium doping zirconic acid lanthanum lithium and silicon doping zirconic acid lanthanum lithium at least
It is a kind of.Preferred embodiment in accordance with the present invention, zirconic acid lanthanum lithium-based ceramic are that tantalum adulterates zirconic acid lanthanum lithium.Chemical stabilization is high as a result, peace
Good perfection.
According to an embodiment of the invention, all-solid lithium-ion battery is in laminated.The each component of battery closely connects as a result,
It touches, is regularly arranged, the interface resistance of battery is smaller.
In accordance with a further aspect of the present invention, the present invention provides a kind of sides for preparing all-solid lithium-ion battery above-mentioned
Method.According to an embodiment of the invention, this method comprises:
(1) composite positive pole slurry and composite negative pole material slurry are prepared, wherein composite positive pole slurry is containing tangible
At the raw material of the predetermined amount of anode layer, composite negative pole material slurry contains the raw material to form the predetermined amount of negative electrode layer, anode composite
The composition and ratio of material slurry and composite negative pole material slurry can be closed by the composition of combination electrode material above-mentioned
The selection and adjustment of reason.
(2) solid-state electrolyte layer is formed, it can be surface-treated solid electrolyte.
(3) composite positive pole slurry and composite negative pole material the slurry shape in the both side surface of solid-state electrolyte layer are utilized
At anode layer and negative electrode layer, i.e., composite positive pole slurry is coated on a side surface of solid-state electrolyte layer, form anode layer,
Composite negative pole material slurry is coated on another side surface of solid-state electrolyte layer, forms negative electrode layer.
(4) it is respectively formed plus plate current-collecting body and negative current collector on the surface of the anode layer and the negative electrode layer, changes sentence
It talks about, exactly forms plus plate current-collecting body on the surface of anode layer, form negative current collector on the surface of negative electrode layer, obtain institute
State all-solid lithium-ion battery.
As a result, using the all-solid lithium-ion battery of this method preparation, security performance is high, and chemical stability is good, output work
Rate is high.
According to an embodiment of the invention, composite positive pole slurry and composite negative pole material slurry are respectively printed at solid-state
It in the both side surface of electrolyte layer and is heat-treated, forms anode layer and negative electrode layer.Anode layer and negative electrode layer are formed as a result,
Process is simple, cost and low energy consumption, is suitble to large-scale production.
According to an embodiment of the invention, solid-state electrolyte layer is ceramic solid electrolyte layer.Output power is high as a result, peace
Good perfection.
Below with reference to specific embodiment, the present invention will be described, it should be noted that these embodiments are only explanation
Property, and be not considered as limiting the invention.
Embodiment 1
Using the method for the embodiment of the present invention, using barium titanate cladding cobalt acid lithium as a positive electrode active material, covering amount
For 5wt.%, the lithium zirconate lanthanum of tantalum doping is as solid electrolyte, and lithium metal is as negative electrode material, assembling solid lithium-ion electric
Pond, the specific steps are as follows:
(1) it is surface-treated the lithium zirconate lanthanum that tantalum adulterates to obtain the solid electrolyte of clean surface；
(2) cobalt acid lithium for coating barium titanate, lithium borate, tin indium oxide conductive additive (mass ratio 6:3:1) are molten respectively
Solution is prepared into anode layer slurry in solvent, and wherein ethyl cellulose is binder, and solvent is butyl carbitol, solid concentration ratio
48wt.%；
(3) by anode layer slurry application to printed in solid electrolyte surface, then 700 degree of heat treatment；(4) using goldleaf as
Plus plate current-collecting body sputters at positive layer surface；
(5) in addition lithium piece is placed directly against solid electrolyte on one side as cathode；
(6) stainless steel collector is attached to lithium piece side as negative current collector；
All-solid-state battery manufactured in the present embodiment is subjected to charge-discharge performance test, the result of charge and discharge at room temperature
As shown in Figure 1, test voltage section is 2.8~4.3V, test electric current is 5uAcm-2。
Embodiment 2
Using the method for the embodiment of the present invention, as a positive electrode active material using pure cobalt acid lithium, the lithium zirconate lanthanum of tantalum doping
As solid electrolyte, lithium metal is as negative electrode material, assembling solid lithium ion battery, the specific steps are as follows:
(1) it is surface-treated the lithium zirconate lanthanum that tantalum adulterates to obtain the solid electrolyte of clean surface；
(2) by lithium cobaltate cathode active material, lithium borate, tin indium oxide conductive additive, lithium fluoride (mass ratio 5:3:1:
1) it is dissolved separately in solvent and is prepared into anode layer slurry, wherein ethyl cellulose is binder, and solvent is butyl carbitol, solid phase
Content ratio 48wt.%
(3) by anode layer slurry application to printed in solid electrolyte surface, then 700 degree of heat treatment；
(4) positive layer surface is sputtered at using goldleaf as plus plate current-collecting body；
(5) in addition lithium piece is placed directly against solid electrolyte on one side as cathode；
(6) stainless steel collector is attached to lithium piece side as negative current collector；
All-solid-state battery manufactured in the present embodiment is subjected to charge-discharge performance test at room temperature, the result of test is such as
Shown in Fig. 2, test voltage section is 2.8~4.3V, and test electric current is 5uAcm-2。
Comparative example
Using the method for the embodiment of the present invention, as a positive electrode active material using cobalt acid lithium, oxide-free nanoparticle, tantalum
The lithium zirconate lanthanum of doping is as solid electrolyte, and lithium metal is as negative electrode material, and assembling solid lithium ion battery, specific steps are such as
Under:
(1) it is surface-treated the lithium zirconate lanthanum that tantalum adulterates to obtain the solid electrolyte of clean surface；
(2) by pure lithium cobaltate cathode active material, lithium borate, tin indium oxide conductive additive, (mass ratio 6:3:1) difference
It is dissolved in solvent and is prepared into anode layer slurry, wherein ethyl cellulose is binder, and solvent is butyl carbitol, solid concentration ratio
48wt.%；
(3) by anode layer slurry application to printed in solid electrolyte surface, then 700 degree of heat treatment；(4) using goldleaf as
Plus plate current-collecting body sputters at positive layer surface；
(5) in addition lithium piece is placed directly against solid electrolyte on one side as cathode；
(6) stainless steel collector is attached to lithium piece side as negative current collector；
All-solid-state battery manufactured in the present embodiment is subjected to charge-discharge performance test at room temperature, the result of test is such as
Shown in Fig. 3, test voltage section is 2.8~4.3V, and test electric current is 5uAcm-2。
The solid Li-ion battery of Examples 1 and 2 is compared with the solid Li-ion battery of comparative example, in surface of active material
The cyclical stability for adding battery after nano oxidized grain significantly improves, after adding inorganic nano-filler inside electrolyte, battery
Discharge capacity significantly improve.
In the description of this specification, reference term " one embodiment ", " some embodiments ", " example ", " specifically show
The description of example " or " some examples " etc. means specific features, structure, material or spy described in conjunction with this embodiment or example
Point is included at least one embodiment or example of the invention.In the present specification, schematic expression of the above terms are not
Centainly refer to identical embodiment or example.Moreover, particular features, structures, materials, or characteristics described can be any
One or more embodiment or examples in can be combined in any suitable manner.
Although an embodiment of the present invention has been shown and described, it will be understood by those skilled in the art that: not
A variety of change, modification, replacement and modification can be carried out to these embodiments in the case where being detached from the principle of the present invention and objective, this
The range of invention is defined by the claims and their equivalents.
Claims (24)
1. a kind of combination electrode material characterized by comprising
Electrode active material, the electrode active material include:
Electrode activity raw material, the electrode activity raw material are positive activated feedstock or negative electrode active raw material；
Oxidate nano grain, the oxidate nano grain are distributed on the surface of the electrode activity raw material；
Clad, the clad are coated on the electrode active material, and the clad includes:
Electrolyte；
Inorganic nano-filler, the inorganic nano-filler are dispersed in the electrolyte；
Conductive agent, the conductive agent are dispersed in the electrolyte,
Wherein, the combination electrode material is in all-solid lithium-ion battery.
2. combination electrode material according to claim 1, which is characterized in that the mass fraction of the clad is 1-
10%.
3. combination electrode material according to claim 1, which is characterized in that the electrolyte, the inorganic nano
The mass ratio of filler and the conductive agent is (10-30): (2-20): (2-20).
4. combination electrode material according to claim 1, which is characterized in that the positive-active raw material is selected from cobalt acid
Lithium, LiMn2O4, nickel-cobalt-manganese ternary material, at least one of nickel ion doped, nickel cobalt manganese richness lithium ternary material and LiFePO4.
5. combination electrode material according to claim 1, which is characterized in that the negative electrode active raw material is selected from carbon substrate
At least one of material, silica-base material, tin-based material, lithium titanate or lithium metal.
6. combination electrode material according to claim 1, which is characterized in that the negative electrode active raw material is lithium metal.
7. combination electrode material according to claim 1, which is characterized in that the oxidate nano grain is selected from Al2O3、
ZrO2、SiO2、BaTiO3、CaTiO3、MgTiO3And MgOAl2O3At least one of.
8. combination electrode material according to claim 1, which is characterized in that the oxidate nano grain is BaTiO3。
9. combination electrode material according to claim 1, which is characterized in that the electrolyte is selected from Li3PO4、
Li4SiO4、Li3BO3、Li4B2O5、LiInO2、Li3InB2O6、LiBO2At least one of.
10. combination electrode material according to claim 1, which is characterized in that the electrolyte is Li3BO3。
11. combination electrode material according to claim 1, which is characterized in that the inorganic nano-filler be selected from LiF,
CaF2、MgF2、LiI、AlF3And LiBF4At least one.
12. combination electrode material according to claim 1, which is characterized in that the inorganic nano-filler is LiF.
13. combination electrode material according to claim 1, which is characterized in that the conductive agent is tin indium oxide, Bi2Te3、
Cu2At least one of Se and BiCuSeO.
14. combination electrode material according to claim 1, which is characterized in that the conductive agent is tin indium oxide.
15. a kind of all-solid lithium-ion battery characterized by comprising
Plus plate current-collecting body；
Anode layer, the anode layer include the described in any item combination electrode materials of claim 1-14, wherein electrode activity is former
Material is positive activated feedstock；
Solid-state electrolyte layer；
Negative electrode layer, the negative electrode layer include the described in any item combination electrode materials of claim 1-14, wherein electrode activity is former
Material is cathode activated feedstock；And
Negative current collector.
16. all-solid lithium-ion battery according to claim 15, which is characterized in that the anode layer with a thickness of 20-
30μm。
17. all-solid lithium-ion battery according to claim 15, which is characterized in that the negative electrode layer with a thickness of 20-
30μm。
18. all-solid lithium-ion battery according to claim 15, which is characterized in that the solid-state electrolyte layer is by zirconium
What sour lanthanum lithium-based ceramic was constituted.
19. all-solid lithium-ion battery according to claim 18, which is characterized in that the zirconic acid lanthanum lithium-based ceramic is choosing
From zirconic acid lanthanum lithium, strontium doping zirconic acid lanthanum lithium, witch culture zirconic acid lanthanum lithium, tantalum doping zirconic acid lanthanum lithium, Ge-doped zirconic acid lanthanum lithium, aluminium doping
At least one of zirconic acid lanthanum lithium and silicon doping zirconic acid lanthanum lithium.
20. all-solid lithium-ion battery according to claim 18, which is characterized in that the zirconic acid lanthanum lithium-based ceramic is tantalum
Adulterate zirconic acid lanthanum lithium.
21. all-solid lithium-ion battery according to claim 15, which is characterized in that the all-solid lithium-ion battery is in
Laminated.
22. a kind of method for preparing the described in any item all-solid lithium-ion batteries of claim 15-21, which is characterized in that packet
It includes:
Composite positive pole slurry and composite negative pole material slurry are prepared, the composite positive pole slurry contains to form anode layer
Predetermined amount raw material, the composite negative pole material slurry contains the raw material to form the predetermined amount of negative electrode layer；
Form solid-state electrolyte layer；
Using the composite positive pole slurry and the composite negative pole material slurry the solid-state electrolyte layer two sides table
Anode layer and negative electrode layer are formed on face；And
It is respectively formed plus plate current-collecting body and negative current collector on the surface of the anode layer and the negative electrode layer, it is described to obtain
All-solid lithium-ion battery.
23. according to the method for claim 22, which is characterized in that by the composite positive pole slurry and the Compound Negative
Pole material slurry is respectively printed in the both side surface of the solid-state electrolyte layer and is heat-treated, and forms anode layer and cathode
Layer.
24. according to the method for claim 22, which is characterized in that the solid-state electrolyte layer is ceramic solid electrolyte
Layer.
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